Urea has been intercalated mechanochemically into dehydrated halloysite and analyzed by X-ray powder diffraction (XRPD), Fourier transform infrared spectroscopy (FTIR), diffuse reflectance ultraviolet/visible spectroscopy (DRUV-VIS), thermal analysis (TGA/DTA), transmission electron microscopy (TEM), and electron paramagnetic resonance (EPR). The basal distance expands from 7.4 to 10.7 angstrom and the interaction of urea to adjacent layers of halloysite through hydrogen bonds increases the structural order of the matrix. After heat treatment in air at different temperatures, decomposition products begin to appear starting from 100 degrees C. Although the basal distance remains constant up to 160 degrees C and collapses to the original value at 200 degrees C, urea and the decomposition products are still present in the sample. Starting from 125 degrees C, urea decomposition products reduce halloysite structural Fe3+ centers to Fe2+, as indicated by DRUV-VIS and EPR spectroscopy. (C) 2009 Elsevier Inc. All rights reserved.